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Title: Non-equilibrium pathways to emergent polar supertextures

Journal Article · · Nature Materials
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [2]; ORCiD logo [5];  [2];  [2];  [6]; ORCiD logo [7];  [8]; ORCiD logo [9];  [2];  [9];  [9];  [9];  [5]; ORCiD logo [10];  [5];  [11] more »;  [11]; ORCiD logo [11];  [11]; ORCiD logo [11]; ORCiD logo [4]; ORCiD logo [12]; ORCiD logo [13]; ORCiD logo [14]; ORCiD logo [6];  [11]; ORCiD logo [2]; ORCiD logo [9]; ORCiD logo [2]; ORCiD logo [9] « less
  1. Pennsylvania State Univ., University Park, PA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); SLAC
  2. Pennsylvania State Univ., University Park, PA (United States)
  3. Indian Institute of Science (IIS) (India)
  4. Argonne National Laboratory (ANL), Argonne, IL (United States)
  5. Japan Synchrotron Radiation Research Institute, Sayo, Hyogo (Japan); RIKEN SPring-8 Center, Sayo (Japan)
  6. Univ. of Tokyo (Japan)
  7. Stanford Univ., CA (United States)
  8. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE)
  9. Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  10. RIKEN SPring-8 Center, Sayo (Japan)
  11. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  12. Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Institute (PULSE); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
  13. University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Rice Univ., Houston, TX (United States)
  14. University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Ultrafast stimuli can stabilize metastable states of matter inaccessible by equilibrium means. Establishing the spatiotemporal link between ultrafast excitation and metastability is crucial to understand these phenomena. Here, in this work, we utilize single-shot optical pump–X-ray probe measurements to capture snapshots of the emergence of a persistent polar vortex supercrystal in a heterostructure that hosts a fine balance between built-in electrostatic and elastic frustrations by design. By perturbing this balance with photoinduced charges, an initially heterogeneous mixture of polar phase disorders within a few picoseconds, leading to a state composed of disordered ferroelectric and suppressed vortex orders. On the picosecond–nanosecond timescales, transient labyrinthine fluctuations develop, accompanied by the recovery of the vortex order. On longer timescales, these fluctuations are progressively quenched by dynamical strain modulations, which drive the collective emergence of a single vortex supercrystal phase. Our results, corroborated by dynamical phase-field modelling, reveal non-equilibrium pathways following the ultrafast excitation of designer systems to persistent metastability.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-05CH11231; AC02-06CH11357; AC02-76SF00515; SC0012375; SC0020145
OSTI ID:
2434005
Journal Information:
Nature Materials, Journal Name: Nature Materials Journal Issue: 10 Vol. 23; ISSN 1476-1122
Publisher:
Springer NatureCopyright Statement
Country of Publication:
United States
Language:
English

References (49)

Tunable Nanoscale Evolution and Topological Phase Transitions of a Polar Vortex Supercrystal journal February 2022
Intrinsic energy band alignment of functional oxides: Intrinsic energy band alignment of functional oxides journal March 2014
Sub-picosecond photo-induced melting of a charge-ordered state in a perovskite manganite journal August 2000
Computing diffraction patterns of microstructures from phase-field simulations journal October 2022
Architecture of Biperovskite-Based LaCrO3/PbTiO3 p–n Heterojunction with a Strong Interface for Enhanced Charge Anti-recombination Process and Visible Light-Induced Photocatalytic Reactions journal December 2018
Thermodynamics of Light-Induced Nanoscale Polar Structures in Ferroelectric Superlattices journal March 2023
Observation of polar vortices in oxide superlattices journal January 2016
Super-crystals in composite ferroelectrics journal February 2016
Cooperative photoinduced metastable phase control in strained manganite films journal July 2016
Phase coexistence and electric-field control of toroidal order in oxide superlattices journal August 2017
Towards properties on demand in quantum materials journal October 2017
A compact X-ray free-electron laser emitting in the sub-ångström region journal June 2012
Phase ordering of charge density waves traced by ultrafast low-energy electron diffraction journal November 2017
Photoinduced multistage phase transitions in Ta2NiSe5 journal April 2021
Dynamical phase-field model of coupled electronic and structural processes journal June 2022
Optical creation of a supercrystal with three-dimensional nanoscale periodicity journal March 2019
Observation of fluctuation-mediated picosecond nucleation of a topological phase journal October 2020
Metal–ferroelectric supercrystals with periodically curved metallic layers journal January 2021
Evidence for topological defects in a photoinduced phase transition journal October 2018
Light-induced charge density wave in LaTe3 journal November 2019
Engineering crystal structures with light journal October 2021
An ultrafast symmetry switch in a Weyl semimetal journal January 2019
Observation of room-temperature polar skyrmions journal April 2019
Inverse transition of labyrinthine domain patterns in ferroelectric thin films journal January 2020
Subterahertz collective dynamics of polar vortices journal April 2021
Observation of the polarization of domains in ferroelectric thin films using x-ray interference journal December 1997
Thermodynamic theory of PbTiO 3 journal October 1987
Development of an X-ray pixel detector with multi-port charge-coupled device for X-ray free-electron laser experiments journal March 2014
How optical excitation controls the structure and properties of vanadium dioxide journal December 2018
Optical Properties and Band Structure of SrTi O 3 and BaTi O 3 journal October 1965
Long-range quadrupole electron-phonon interaction from first principles journal September 2020
Surface generation and detection of phonons by picosecond light pulses journal September 1986
Photoinduced Melting of Antiferromagnetic Order in La 0.5 Sr 1.5 MnO 4 Measured Using Ultrafast Resonant Soft X-Ray Diffraction journal May 2011
Ultrafast Photovoltaic Response in Ferroelectric Nanolayers journal February 2012
Mesoscopic Free Path of Nonthermalized Photogenerated Carriers in a Ferroelectric Insulator journal March 2017
Dynamics of a Persistent Insulator-to-Metal Transition in Strained Manganite Films journal December 2019
Effect of Mechanical Boundary Conditions on Phase Diagrams of Epitaxial Ferroelectric Thin Films journal March 1998
Coupled Ultrafast Lattice and Polarization Dynamics in Ferroelectric Nanolayers journal June 2007
Colloquium: Nonthermal pathways to ultrafast control in quantum materials journal October 2021
Topological phases in polar oxide nanostructures journal April 2023
Controlling the metal-to-insulator relaxation of the metastable hidden quantum state in 1T-TaS 2 journal July 2015
Atomic mapping of periodic dipole waves in ferroelectric oxide journal July 2021
Snapshots of a light-induced metastable hidden phase driven by the collapse of charge order journal July 2022
Light-Induced Superconductivity in a Stripe-Ordered Cuprate journal January 2011
Ultrafast Switching to a Stable Hidden Quantum State in an Electronic Crystal journal April 2014
Ultrafast disordering of vanadium dimers in photoexcited VO 2 journal November 2018
Femtosecond x-ray diffraction reveals a liquid–liquid phase transition in phase-change materials journal June 2019
Terahertz field–induced ferroelectricity in quantum paraelectric SrTiO 3 journal June 2019
Enhanced charge density wave coherence in a light-quenched, high-temperature superconductor journal May 2022